A machine-learning-enabled smart neckband for monitoring dietary intake.

The increasing need for precise dietary monitoring across various health scenarios has led to innovations in wearable sensing technologies. However, continuously tracking food and fluid intake during daily activities can be complex. In this study, we present a machine-learning-powered smart neckband that features wireless connectivity and a comfortable, foldable design. Initially considered beneficial for managing conditions such as diabetes and obesity by facilitating dietary control, the device's utility extends beyond these applications. It has proved to be valuable for sports enthusiasts, individuals focused on diet control, and general health monitoring. Its wireless connectivity, ergonomic design, and advanced classification capabilities offer a promising solution for overcoming the limitations of traditional dietary tracking methods, highlighting its potential in personalized healthcare and wellness strategies.

Transparent radiative cooling cover window for flexible and foldable electronic displays.

Transparent radiative cooling holds the promise to efficiently manage thermal conditions in various electronic devices without additional energy consumption. Radiative cooling cover windows designed for foldable and flexible displays could enhance cooling capacities in the ubiquitous deployment of flexible electronics in outdoor environments. However, previous demonstrations have not met the optical, mechanical, and moisture-impermeable criteria for such cover windows. Herein, we report transparent radiative cooling metamaterials with a thickness of 50 microns as a cover window of foldable and flexible displays by rational design and synthesis of embedding optically-modulating microstructures in clear polyimide. The resulting outcome not only includes excellent light emission in the atmospheric window under the secured optical transparency but also provides enhanced mechanical and moisture-impermeable properties to surpass the demands of target applications. Our metamaterials not only substantially mitigate the temperature rise in heat-generating devices exposed to solar irradiance but also enhance the thermal management of devices in dark conditions. The light output performance of light-emitting diodes in displays on which the metamaterials are deployed is greatly enhanced by suppressing the performance deterioration associated with thermalization.

Spongy Ag Foam for Soft and Stretchable Strain Gauges.

Strain gauges, particularly for wearable sensing applications, require a high degree of stretchability, softness, sensitivity, selectivity, and linearity. They must also steer clear of challenges such as mechanical and electrical hysteresis, overshoot behavior, and slow response/recovery times. However, current strain gauges face challenges in satisfying all of these requirements at once due to the inevitable trade-offs between these properties. Here, we present an innovative method for creating strain gauges from spongy Ag foam through a steam-etching process. This method simplifies the traditional, more complex, and costly manufacturing techniques, presenting an eco-friendly alternative. Uniquely, the strain gauges crafted from this method achieve an unparalleled gauge factor greater than 8 × 103 at strains exceeding 100%, successfully meeting all required attributes without notable trade-offs. Our work includes systematic investigations that reveal the intricate structure-property-performance relationship of the spongy Ag foam with practical demonstrations in areas such as human motion monitoring and human-robot interaction. These breakthroughs pave the way for highly sensitive and selective strain gauges, showing immediate applicability across a wide range of wearable sensing applications.

Rapid Self-Healing Hydrogel with Ultralow Electrical Hysteresis for Wearable Sensing.

Self-healing hydrogels are in high demand for wearable sensing applications due to their remarkable deformability, high ionic and electrical conductivity, self-adhesiveness to human skin, as well as resilience to both mechanical and electrical damage. However, these hydrogels face challenges such as delayed healing times and unavoidable electrical hysteresis, which limit their practical effectiveness. Here, we introduce a self-healing hydrogel that exhibits exceptionally rapid healing with a recovery time of less than 0.12 s and an ultralow electrical hysteresis of less than 0.64% under cyclic strains of up to 500%. This hydrogel strikes an ideal balance, without notable trade-offs, between properties such as softness, deformability, ionic and electrical conductivity, self-adhesiveness, response and recovery times, durability, overshoot behavior, and resistance to nonaxial deformations such as twisting, bending, and pressing. Owing to this unique combination of features, the hydrogel is highly suitable for long-term, durable use in wearable sensing applications, including monitoring body movements and electrophysiological activities on the skin.

Transparent Intracellular Sensing Platform with Si Needles for Simultaneous Live Imaging.

Vertically ordered Si needles are of particular interest for long-term intracellular recording owing to their capacity to infiltrate living cells with negligible damage and minimal toxicity. Such intracellular recordings could greatly benefit from simultaneous live cell imaging without disrupting their culture, contributing to an in-depth understanding of cellular function and activity. However, the use of standard live imaging techniques, such as inverted and confocal microscopy, is currently impeded by the opacity of Si wafers, typically employed for fabricating vertical Si needles. Here, we introduce a transparent intracellular sensing platform that combines vertical Si needles with a percolated network of Au-Ag nanowires on a transparent elastomeric substrate. This sensing platform meets all prerequisites for simultaneous intracellular recording and imaging, including electrochemical impedance, optical transparency, mechanical compliance, and cell viability. Proof-of-concept demonstrations of this sensing platform include monitoring electrical potentials in cardiomyocyte cells and in three-dimensionally engineered cardiovascular tissue, all while conducting live imaging with inverted and confocal microscopes. This sensing platform holds wide-ranging potential applications for intracellular research across various disciplines such as neuroscience, cardiology, muscle physiology, and drug screening.

In Situ Spray Polymerization of Conductive Polymers for Personalized E-textiles.

E-textiles, also known as electronic textiles, seamlessly merge wearable technology with fabrics, offering comfort and unobtrusiveness and establishing a crucial role in health monitoring systems. In this field, the integration of custom sensor designs with conductive polymers into various fabric types, especially in large areas, has presented significant challenges. Here, we present an innovative additive patterning method that utilizes a dual-regime spray system, eliminating the need for masks and allowing for the programmable inscription of sensor arrays onto consumer textiles. Unlike traditional spray techniques, this approach enables in situ, on-the-fly polymerization of conductive polymers, enabling intricate designs with submillimeter resolution across fabric areas spanning several meters. Moreover, it addresses the nozzle clogging issues commonly encountered in such applications. The resulting e-textiles preserve essential fabric characteristics such as breathability, wearability, and washability while delivering exceptional sensing performance. A comprehensive investigation, combining experimental, computational, and theoretical approaches, was conducted to examine the critical factors influencing the operation of the dual-regime spraying system and its role in e-textile fabrication. These findings provide a flexible solution for producing e-textiles on consumer fabric items and hold significant implications for a diverse range of wearable sensing applications.

Biodegradable silicon nanoneedles for ocular drug delivery.

Ocular drug delivery remains a grand challenge due to the complex structure of the eye. Here, we introduce a unique platform of ocular drug delivery through the integration of silicon nanoneedles with a tear-soluble contact lens. The silicon nanoneedles can penetrate into the cornea in a minimally invasive manner and then undergo gradual degradation over the course of months, enabling painless and long-term sustained delivery of ocular drugs. The tear-soluble contact lens can fit a variety of corneal sizes and then quickly dissolve in tear fluid within a minute, enabling an initial burst release of anti-inflammatory drugs. We demonstrated the utility of this platform in effectively treating a chronic ocular disease, such as corneal neovascularization, in a rabbit model without showing a notable side effect over current standard therapies. This platform could also be useful in treating other chronic ocular diseases.

Genome-Scale Analysis of Acetobacterium woodii Identifies Translational Regulation of Acetogenesis.

Acetogens synthesize acetyl-CoA via the CO2-fixing Wood-Ljungdahl pathway. Despite their ecological and biotechnological importance, their translational regulation of carbon and energy metabolisms remains unclear. Here, we report how carbon and energy metabolisms in the model acetogen Acetobacterium woodii are translationally controlled under different growth conditions. Data integration of genome-scale transcriptomic and translatomic analyses revealed that the acetogenesis genes, including those of the Wood-Ljungdahl pathway and energy metabolism, showed changes in translational efficiency under autotrophic growth conditions. In particular, genes encoding the Wood-Ljungdahl pathway are translated at similar levels to achieve efficient acetogenesis activity under autotrophic growth conditions, whereas genes encoding the carbonyl branch present increased translation levels in comparison to those for the methyl branch under heterotrophic growth conditions. The translation efficiency of genes in the pathways is differentially regulated by 5' untranslated regions and ribosome-binding sequences under different growth conditions. Our findings provide potential strategies to optimize the metabolism of syngas-fermenting acetogenic bacteria for better productivity. IMPORTANCE Acetogens are capable of reducing CO2 to multicarbon compounds (e.g., ethanol or 2,3-butanediol) via the Wood-Ljungdahl pathway. Given that protein synthesis in bacteria is highly energy consuming, acetogens living at the thermodynamic limit of life are inevitably under translation control. Here, we dissect the translational regulation of carbon and energy metabolisms in the model acetogen Acetobacterium woodii under heterotrophic and autotrophic growth conditions. The latter may be experienced when acetogen is used as a cell factory that synthesizes products from CO2 during the gas fermentation process. We found that the methyl and carbonyl branches of the Wood-Ljungdahl pathway are activated at similar translation levels during autotrophic growth. Translation is mainly regulated by the 5'-untranslated-region structure and ribosome-binding-site sequence. This work reveals novel translational regulation for coping with autotrophic growth conditions and provides the systematic data set, including the transcriptome, translatome, and promoter/5'-untranslated-region bioparts.

Rapid custom prototyping of soft poroelastic biosensor for simultaneous epicardial recording and imaging.

The growing need for the implementation of stretchable biosensors in the body has driven rapid prototyping schemes through the direct ink writing of multidimensional functional architectures. Recent approaches employ biocompatible inks that are dispensable through an automated nozzle injection system. However, their application in medical practices remains challenged in reliable recording due to their viscoelastic nature that yields mechanical and electrical hysteresis under periodic large strains. Herein, we report sponge-like poroelastic silicone composites adaptable for high-precision direct writing of custom-designed stretchable biosensors, which are soft and insensitive to strains. Their unique structural properties yield a robust coupling to living tissues, enabling high-fidelity recording of spatiotemporal electrophysiological activity and real-time ultrasound imaging for visual feedback. In vivo evaluations of custom-fit biosensors in a murine acute myocardial infarction model demonstrate a potential clinical utility in the simultaneous intraoperative recording and imaging on the epicardium, which may guide definitive surgical treatments.

Replicable Quasi-Three-Dimensional Plasmonic Nanoantennas for Infrared Bandpass Filtering.

Quasi-three-dimensionally designed metal-dielectric hybrid nanoantennas have provided a unique capability to control light at the nanoscale beyond the diffraction limit, which has enabled powerful optical manipulation techniques. However, the fabrication of these nanoantennas has largely relied on the use of nanolithography techniques that are time- and cost-consuming, impeding their application in wide-ranging use. Herein, we report a versatile methodology enabling the repetitive replication of these nanoantennas from their silicon molds with tailored optical features for infrared bandpass filtering. Comprehensive experimental and computational analyses revealed the underlying mechanism of this methodology and also provided a technical guideline for pragmatic translation into infrared filters in multispectral imaging.

Controlled Integration of Interconnected Pores under Polymeric Surfaces for Low Adhesion and Antiscaling Performance.

Low-adhesive surfaces have been highlighted due to the potentials to mitigate fouling issues by preventing unwanted substances from adhering. Realizing superhydrophobicity with 3D surface structures/chemical modifiers or fabricating lubricant-assisted slippery surfaces has been demonstrated to realize low-adhesive surfaces. However, they still need to overcome the transition to Wenzel from Cassie states of droplets on 3D surface structures or the lubricant depletion issues of slippery surfaces for sustainable operations. Herein, we report the fabrication of low-adhesive polymeric surfaces, neither assisted by 3D surface structures/chemical modifiers nor lubricants, which is realized by embedding the interconnected pore networks underneath the top smooth surface using a water steaming method. The fabricated silicone surfaces exhibit low-adhesive properties due to the stress concentration effects generated by the subsurface-structured pores, favorable for easy detachment of the adherent from the surface. Our platform can be exploited to lower adhesion of superhydrophilic surfaces or to achieve ultralow-adhesive properties upon combination with superhydrophobicity. Finally, scale precipitation tests reveal 4.2 times lower scale accumulation of our low-adhesive polymeric surfaces than that in control samples.

Acetogenic bacteria utilize light-driven electrons as an energy source for autotrophic growth.

Acetogenic bacteria use cellular redox energy to convert CO2 to acetate using the Wood-Ljungdahl (WL) pathway. Such redox energy can be derived from electrons generated from H2 as well as from inorganic materials, such as photoresponsive semiconductors. We have developed a nanoparticle-microbe hybrid system in which chemically synthesized cadmium sulfide nanoparticles (CdS-NPs) are displayed on the cell surface of the industrial acetogen Clostridium autoethanogenum The hybrid system converts CO2 into acetate without the need for additional energy sources, such as H2, and uses only light-induced electrons from CdS-NPs. To elucidate the underlying mechanism by which C. autoethanogenum uses electrons generated from external energy sources to reduce CO2, we performed transcriptional analysis. Our results indicate that genes encoding the metal ion or flavin-binding proteins were highly up-regulated under CdS-driven autotrophic conditions along with the activation of genes associated with the WL pathway and energy conservation system. Furthermore, the addition of these cofactors increased the CO2 fixation rate under light-exposure conditions. Our results demonstrate the potential to improve the efficiency of artificial photosynthesis systems based on acetogenic bacteria integrated with photoresponsive nanoparticles.

3D Printed Bioresponsive Devices with Selective Permeability Inspired by Eggshell Membrane for Effective Biochemical Conversion.

Eggshell membrane has selective permeability that enables gas or liquid molecules to pass through while effectively preventing migration of microbial species. Herein, inspired by the architecture of the eggshell membrane, we employ three-dimensional (3D) printing techniques to realize bioresponsive devices with excellent selective permeability for effective biochemical conversion. The fabricated devices show 3D conductive carbon nanofiber membranes in which precultured microbial cells are controllably deployed. The resulting outcome provides excellent selective permeability between chemical and biological species, which enables acquisition of target responses generated by biological species confined within the device upon input signals. In addition, electrically conductive carbon nanofiber networks provide a platform for real-time monitoring of metabolism of microbial cells in the device. The suggested platform represents an effort to broaden microbial applications by constructing biologically programmed devices for desired responses enabled by designated deployment of engineered cells in a securely confined manner within enclosed membranes using 3D printing methods.

Bactericidal Lubricating Synthetic Materials for Three-Dimensional Additive Assembly with Controlled Mechanical Properties.

3D printable synthetic materials have been developed to realize desired surface and mechanical properties. Lubricating synthetic surfaces have broad technological impacts on many applications including food packaging, microfluidic systems, and biomedical devices. However, combining soft materials with lubricants leads to significant phase separation and swelling phenomena, together with lowered mechanical strength, impeding full utilization of lubricating synthetic surfaces with desired shapes in a highly controllable manner. Here, we report a new platform to create a 3D printable lubricant-polymer composite (3D-LUBRIC) for the seamless fabrication of multidimensional structures with diverse functionalities. The rationally designed lubricant-polymer mixtures including silica aerogel particles not only exhibit suitable rheological properties for direct ink writing without phase separation but also enable the deterministic additive assembly of heterogeneous materials, which have large mismatches of oil permeability, with no distinct shape distortion. While exhibiting excellent lubricating properties for a variety of liquids, 3D-LUBRIC shows tunable mechanical properties with desired functionalities, such as optical transparency, flexibility and stretchability, and anti-icing and antibacterial/bactericidal properties. We employ the proposed platform to fabricate self-cleanable containers and antibacterial/bactericidal medical tubes. Our platform can offer new opportunities for building low-adhesive, multifunctional synthetic materials with customized shapes for diverse applications.

Bioresorbable, Miniaturized Porous Silicon Needles on a Flexible Water-Soluble Backing for Unobtrusive, Sustained Delivery of Chemotherapy.

Conventional melanoma therapies suffer from the toxicity and side effects of repeated treatments due to the aggressive and recurrent nature of melanoma cells. Less-invasive topical chemotherapies by utilizing polymeric microneedles have emerged as an alternative, but the sustained, long-lasting release of drug cargos remains challenging. In addition, the size of the microneedles is relatively bulky for the small, curvilinear, and exceptionally sensitive cornea for the treatment of ocular melanoma. Here, we report a design of bioresorbable, miniaturized porous-silicon (p-Si) needles with covalently linked drug cargos at doses comparable to those of conventional polymeric microneedles. The p-Si needles are built on a water-soluble film as a temporary flexible holder that can be intimately interfaced with the irregular surface of living tissues, followed by complete dissolution with saline solution within 1 min. Consequently, the p-Si needles remain embedded inside tissues and then undergo gradual degradation, allowing for sustained release of the drug cargos. Its utility in unobtrusive topical delivery of chemotherapy with minimal side effects is demonstrated in a murine melanoma model.

Adaptive Laboratory Evolution of Eubacterium limosum ATCC 8486 on Carbon Monoxide.

Acetogens are naturally capable of metabolizing carbon monoxide (CO), a component of synthesis gas (syngas), for autotrophic growth in order to produce biomass and metabolites such as acetyl-CoA via the Wood-Ljungdahl pathway. However, the autotrophic growth of acetogens is often inhibited by the presence of high CO concentrations because of CO toxicity, thus limiting their biosynthetic potential for industrial applications. Herein, we implemented adaptive laboratory evolution (ALE) for growth improvement of Eubacterium limosum ATCC 8486 under high CO conditions. The strain evolved under syngas conditions with 44% CO over 150 generations, resulting in a significant increased optical density (600 nm) and growth rate by 2.14 and 1.44 folds, respectively. In addition, the evolved populations were capable of proliferating under CO concentrations as high as 80%. These results suggest that cell growth is enhanced as beneficial mutations are selected and accumulated, and the metabolism is altered to facilitate the enhanced phenotype. To identify the causal mutations related to growth improvement under high CO concentrations, we performed whole genome resequencing of each population at 50-generation intervals. Interestingly, we found key mutations in CO dehydrogenase/acetyl-CoA synthase (CODH/ACS) complex coding genes, acsA and cooC. To characterize the mutational effects on growth under CO, we isolated single clones and confirmed that the growth rate and CO tolerance level of the single clone were comparable to those of the evolved populations and wild type strain under CO conditions. Furthermore, the evolved strain produced 1.34 folds target metabolite acetoin when compared to the parental strain while introducing the biosynthetic pathway coding genes to the strains. Consequently, this study demonstrates that the mutations in the CODH/ACS complex affect autotrophic growth enhancement in the presence of CO as well as the CO tolerance of E. limosum ATCC 8486.

Functional cooperation of the glycine synthase-reductase and Wood-Ljungdahl pathways for autotrophic growth of Clostridium drakei.

Among CO2-fixing metabolic pathways in nature, the linear Wood-Ljungdahl pathway (WLP) in phylogenetically diverse acetate-forming acetogens comprises the most energetically efficient pathway, requires the least number of reactions, and converts CO2 to formate and then into acetyl-CoA. Despite two genes encoding glycine synthase being well-conserved in WLP gene clusters, the functional role of glycine synthase under autotrophic growth conditions has remained uncertain. Here, using the reconstructed genome-scale metabolic model iSL771 based on the completed genome sequence, transcriptomics, 13C isotope-based metabolite-tracing experiments, biochemical assays, and heterologous expression of the pathway in another acetogen, we discovered that the WLP and the glycine synthase pathway are functionally interconnected to fix CO2, subsequently converting CO2 into acetyl-CoA, acetyl-phosphate, and serine. Moreover, the functional cooperation of the pathways enhances CO2 consumption and cellular growth rates via bypassing reducing power required reactions for cellular metabolism during autotrophic growth of acetogens.

Genome Engineering of Eubacterium limosum Using Expanded Genetic Tools and the CRISPR-Cas9 System.

Eubacterium limosum is one of the important bacteria in C1 feedstock utilization as well as in human gut microbiota. Although E. limosum has recently garnered much attention and investigation on a genome-wide scale, a bottleneck for systematic engineering in E. limosum is the lack of available genetic tools and an efficient genome editing platform. To overcome this limitation, we here report expanded genetic tools and the CRISPR-Cas9 system. We have developed an inducible promoter system that enables implementation of the CRISPR-Cas9 system to precisely manipulate target genes of the Wood-Ljungdahl pathway with 100% efficiency. Furthermore, we exploited the effectiveness of CRISPR interference to reduce the expression of target genes, exhibiting substantial repression of several genes in the Wood-Ljungdahl pathway and fructose-PTS system. These expanded genetic tools and CRISPR-Cas9 system comprise powerful and widely applicable genetic tools to accelerate functional genomic study and genome engineering in E. limosum.

Sensor-Instrumented Scaffold Integrated with Microporous Spongelike Ultrabuoy for Long-Term 3D Mapping of Cellular Behaviors and Functions.

Real-time monitoring of cellular behaviors and functions with sensor-instrumented scaffolds can provide a profound impact on fundamental studies of the underlying biophysics and disease modeling. Although quantitative measurement of predictive data for in vivo tests and physiologically relevant information in these contexts is important, the long-term reliable monitoring of cellular functions in three-dimensional (3D) environments is limited by the required set under wet cell culture conditions that are unfavorable to electronic instrument settings. Here, we introduce an ultrabuoyant 3D instrumented scaffold that can remain afloat on the surface of culture medium and thereby provides favorable environments for the entire electronic components in the air while the cells reside and grow underneath. This setting enables high-fidelity recording of electrical cell-substrate impedance and electrophysiological signals for a long period of time (weeks). Comprehensive in vitro studies reveal the utility of this platform as an effective tool for drug screening and tissue development.

Hierarchical Macroporous Particles for Efficient Whole-Cell Immobilization: Application in Bioconversion of Greenhouse Gases to Methanol.

A viable approach for methanol production under ambient physiological conditions is to use greenhouse gases, methane (CH4) and carbon dioxide (CO2), as feed for immobilized methanotrophs. In the present study, unique macroporous carbon particles with pore sizes in the range of ∼1-6 µm were synthesized and used as support for the immobilization of Methylocella tundrae. Immobilization was accomplished covalently on hierarchical macroporous carbon particles. Maximal cell loading of covalently immobilized M. tundrae was 205 mgDCM g-1 of particles. Among these particles, the cells immobilized on 3.6 µm pore size particles showed the highest reusability with the least leaching and were chosen for further study. After immobilization, M. tundrae showed up to 2.4-fold higher methanol production stability at various pH and temperature values because of higher stability and metabolic activity than free cells. After eight cycles of reuse, the immobilized cells retained 18.1-fold higher relative production stability compared to free cells. Free and immobilized cells exhibited cumulative methanol production of 5.2 and 9.5 µmol mgDCM-1 under repeated batch conditions using simulated biogas [CH4 and CO2, 4:1 (v/v)] as feed, respectively. The appropriate pore size of macroporous particles favors the efficient M. tundrae immobilization to retain better biocatalytic properties. This is the first report concerning the covalent immobilization of methanotrophs on the newly synthesized macroporous carbon particles and its subsequent application in repeated methanol production using simulated biogas as a feed.